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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Grain‐Boundary‐Rich Noble Metal Nanoparticle Assemblies: Synthesis, Characterization, and Reactivity

Abstract Here, a comprehensive study on the synthesis, characterization, and reactivity of grain‐boundary (GB)‐rich noble metal nanoparticle (NP) assemblies is presented. A facile and scalable synthesis of Pt, Pd, Au, Ag, and Rh NP assemblies is developed, in which NPs are predominantly connected via Σ3 (111) twin GBs, forming a network. Driven by water electrolysis, the random collisions and oriented attachment of colloidal NPs in solution lead to the formation of Σ3 (111) twin boundaries and some highly mismatched GBs. This synthetic method also provides convenient control over the GB density without altering the crystallite size or GB type by varying the NP collision frequency. The structural characterization reveals the presence of localized tensile strain at the GB sites. The ultrahigh activity of GB‐rich Pt NP assembly toward catalytic hydrogen oxidation in air is demonstrated, enabling room‐temperature catalytic hydrogen sensing for the first time. Finally, density functional theory calculations reveal that the strained Σ3(111) twin boundary facilitates oxygen dissociation, drastically enhancing the hydrogen oxidation rate via the dissociative pathway. This reported large‐scale synthesis of the Σ3 (111) twin GB‐rich structures enables the development of a broad range of high‐performance GB‐rich catalysts.

Geng, Xin↗
NASA NTRS2017

Metallized Nanotube Polymer Composite (MNPC) and Methods for Making Same

A novel method to develop highly conductive functional materials which can effectively shield various electromagnetic effects (EMEs) and harmful radiations. Metallized nanotube polymer composites (MNPC) are composed of a lightweight polymer matrix, superstrong nanotubes (NT), and functional nanoparticle inclusions. MNPC is prepared by supercritical fluid infusion of various metal precursors (Au, Pt, Fe, and Ni salts), incorporated simultaneously or sequentially, into a solid NT-polymer composite followed by thermal reduction. The infused metal precursor tends to diffuse toward the nanotube surface preferentially as well as the surfaces of the NT-polymer matrix, and is reduced to form nanometer-scale metal particles or metal coatings. The conductivity of the MNPC increases with the metallization, which provides better shielding capabilities against various EMEs and radiations by reflecting and absorbing EM waves more efficiently. Furthermore, the supercritical fluid infusion process aids to improve the toughness of the composite films significantly regardless of the existence of metal.

Park, Cheol↗
DOE OSTI2020

Biomimetic Catalysts Based on Au@ZnO–Graphene Composites for the Generation of Hydrogen by Water Splitting

For some decades, the scientific community has been looking for alternatives to the use of fossil fuels that allow for the planet’s sustainable and environmentally-friendly development. To do this, attempts have been made to mimic some processes that occur in nature, among which the photosystem-II stands out, which allows water splitting operating with different steps to generate oxygen and hydrogen. This research presents promising results using synthetic catalysts, which try to simulate some natural processes, and which are based on Au@ZnO–graphene compounds. These catalysts were prepared by incorporating different amounts of gold nanoparticles (1 wt.%, 3 wt.%, 5 wt.%, 10 wt.%) and graphene (1 wt.%) on the surface of synthesized zinc oxide nanowires (ZnO NWs), and zinc oxide nanoparticles (ZnO NPs), along with a commercial form (commercial ZnO) for comparison purposes. The highest amount of hydrogen (1127 μmol/hg) was reported by ZnO NWs with a gold and graphene loadings of 10 wt.% and 1 wt.%, respectively, under irradiation at 400 nm. Quantities of 759 μmol/hg and 709 μmol/hg were obtained with catalysts based on ZnO NPs and commercial ZnO, respectively. The photocatalytic activity of all composites increased with respect to the bare semiconductors, being 2.5 times higher in ZnO NWs, 8.8 times higher for ZnO NPs, and 7.5 times higher for commercial ZnO. The high photocatalytic activity of the catalysts is attributed, mainly, to the synergism between the different amount of gold and graphene incorporated, and the surface area of the composites.

Machín, Abniel (ORCID:0000000341343344)↗
DOE OSTI2022

Method for preparation of nanoceria supported atomic noble metal catalysts and the application of platinum single atom catalysts for direct methane conversion

Described are methods for converting methane to olefins, aromatics, or a combination thereof using a single atom catalyst comprising CeO2 nanoparticles impregnated with individual atoms of noble metals including Pt, Pd, Rh, Ru, Ag, Au, Ir, or a combination thereof. These single atom catalysts of the present invention are heated with methane to form olefins and aromatics.

Wang, Chao↗
DOE OSTI2022

Z-Contrast Enhancement in Au–Pt Nanocatalysts by Correlative X-ray Absorption Spectroscopy and Electron Microscopy: Implications for Composition Determination

The properties of bimetallic nanoparticles (BNPs) vary widely as a function of their composition and size distributions. X-ray absorption fine structure analysis is commonly used to characterize their structure, but its application to elements that are close to each other in the periodic table is hampered by poor Z-contrast. For this study, we trained an artificial neural network to recognize the partial coordination numbers in AuPt NPs synthesized via peptide templating using their X-ray absorption near-edge structure spectra. This approach, combined with scanning transmission electron microscopy analysis, revealed unique details of this prototype catalytic system that has different forms of heterogeneities at both the intra- and inter-particle levels. Our method based on the enhancement of Z-contrast of metal species will have implications for compositional studies of BNPs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Ultimate compressive strength and severe plastic deformation of equilibrated single-crystalline copper nanoparticles

Mechanical properties and deformation mechanisms of defect-free copper nanoparticles are investigated by combining experiments with atomistic simulations. The compressive strength of the particles increases with decreasing size and tends to saturate near the theoretical strength in the small-size limit. In this limit, the intrinsic size dependence of the strength is governed by the stochastic nature of dislocation nucleation near the particle surface. The particle deformation process evolves from the initial strain softening to strain hardening as the particle accumulates residual damage. The normalized strength-size relation for Cu is compared with those for Au, Ni, and Pt. The lack of universal behavior among the four FCC metals is discussed. Heavily deformed Cu nanoparticles develop polycrystalline structures and change the lattice orientation from [111] to [110]. The experiments and simulations reveal the twinning mechanism of the lattice rotation leading to the new grain formation.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ultimate compressive strength and severe plastic deformation of equilibrated single-crystalline copper nanoparticles

Mechanical properties and deformation mechanisms of defect-free copper nanoparticles are investigated by combining experiments with atomistic simulations. The compressive strength of the particles increases with decreasing size and tends to saturate near the theoretical strength in the small-size limit. In this limit, the intrinsic size dependence of the strength is governed by the stochastic nature of dislocation nucleation near the particle surface. The particle deformation process evolves from the initial strain softening to strain hardening as the particle accumulates residual damage. The normalized strength-size relation for Cu is compared with those for Au, Ni, and Pt. The lack of universal behavior among the four FCC metals is discussed. Heavily deformed Cu nanoparticles develop polycrystalline structures and change the lattice orientation from [111] to [110]. The experiments and simulations reveal the twinning mechanism of the lattice rotation leading to the new grain formation.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Unraveling 1-Hexene Hydrogenation over Dilute Pd-in-Au Alloys

Dilute Pd-in-Au alloys are valuable materials for selectively hydrogenating alkynes and isomerizing alkenes. By diluting Pd in a Au host, the selectivity toward semihydrogenated alkene isomers can be significantly enhanced and the unfavorable overhydrogenation to alkanes is suppressed. However, a detailed mechanistic study on the origin of the enhanced alkene selectivity over dilute alloy catalysts is still missing. Here, we combine experiment and theory to unravel the reaction mechanism, identifying rate-limiting and selectivity-controlling steps in 1-hexene hydrogenation over dilute Pd-in-Au catalysts. Using isotope-exchange hydrogenation experiments, we show that 1-hexene and hydrogen over a bimetallic Pd4Au96 in silica catalyst preferentially form 1-hexene isomers, (trans and cis) 2- and 3-hexene and only a small amounts of hexane. The reaction is consistent with a Horiuti–Polanyi mechanism, similar to a monometallic Pd nanoparticle catalyst. Computation of the free-energy profiles for 1-hexene hydrogenation and isomerization over a single Pd atom in a Au surface using first principles calculations indicated that the isomerization of 1-hexene to 2-hexene is energetically favorable due to the relatively large barrier for H2 dissociation preventing hydrogenation to n-hexane. Microkinetic modeling established that H2 dissociation on the single-atom Pd sites and H spillover from these sites onto the Au host are rate-limiting and key in steering the selectivity of dilute Pd-in-Au alloys toward the hexene isomers. Furthermore, the mechanistic insights from this study contribute to the rational design of optimized dilute alloy catalysts for selective alkene isomerization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Laser pulse induced second- and third-harmonic generation of gold nanorods with real-time time-dependent density functional tight binding (RT-TDDFTB) method

In this paper, we investigate second- and third-harmonic generation processes in Au nanorod systems using the real-time time-dependent density functional tight binding method. Our study focuses on the computation of nonlinear signals based on the time dependent dipole response induced by linearly polarized laser pulses interacting with nanoparticles. We systematically explore the influence of various laser parameters, including pump intensity, duration, frequency, and polarization directions, on harmonic generation. We demonstrate all the results using Au nanorod dimer systems arranged in end-to-end configurations, and disrupting the spatial symmetry of regular single nanorod systems is crucial for second-harmonic generation processes. Furthermore, we study the impact of nanorod lengths, which lead to variable plasmon energies, on harmonic generation, and estimates of polarizabilities and hyper-polarizabilities are provided.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Anions in Corrosion: Influence of Polymer Electrolytes on the Interfacial Ion Transfer Kinetics of Cu at Au(111) Surfaces

The corrosion kinetics of metals in the presence of polymer electrolytes—which are often used in devices for the electrochemical production of hydrogen, hydrocarbons, and alcohols—is convoluted by transport and ill-defined reactive interfaces which mask the fundamental reaction kinetics. Underpotential-deposited monolayers of Cu at Au(111) surfaces provide a structurally welldefined active site for interfacial ion transfer, with a fixed number of sites available for adsorption. Here, we investigate the adsorption behavior of Cu at Au(111) surfaces across a series of sulfate and sulfonate electrolytes, to understand how anion structure influences the kinetics of elementary interfacial ion-transfer reactions. The influence of anion structure is most significant at high adsorbate coverage, with similar adsorption isotherms and kinetics observed for all three molecular sulfates and sulfonates. In contrast, a suspended perfluorosulfonic acid ionomer reduced both the equilibrium coverage of Cu as well as the standard exchange rate at Au(111) at low coverages of Cu. These results suggest that electrocatalyst corrosion is inhibited for metal nanoparticles supported at polymer electrolytes due to changes in adsorbate coverage as well as suppressed kinetics for interfacial ion transfer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Electronic relaxation dynamics in [Au 25 (SR) 18 ] -1 (R = CH 3 , C 2 H 5 , C 3 H 7 , MPA, PET) thiolate-protected nanoclusters

Here we investigate the excited electron dynamics in [Au 25 (SR) 18 ] -1 (R = CH3, C 2 H 5 , C 3 H 7 , MPA, PET) [MPA = mercaptopropanoic acid, PET = phenylethylthiol] nanoparticles to understand how different ligands affect the excited state dynamics in this system. The population dynamics of the core and higher excited states lying in the energy range 0.00–2.20 eV are studied using a surface hopping method with decoherence correction in a real-time DFT approach. All of the ligated clusters follow a similar trend in decay for the core states (S 1 –S 6 ). The observed time constants are on the picosecond time scale (2–19 ps), which agrees with the experimental time scale, and this study confirms that the time constants observed experimentally could originate from core-to-core transitions and not from core-to-semiring transitions. In the presence of higher excited states, R = H, CH 3 , C 2 H 5 , C 3 H 7 , and PET demonstrate similar relaxations trends whereas R = MPA shows slightly different relaxation of the core states due to a smaller gap between the LUMO+1 and LUMO+2 gap in its electronic structure. The S 1 (HOMO → LUMO) state gives the slowest decay in all ligated clusters, while S 7 has a relatively long decay. Furthermore, separate electron and hole relaxations were performed on the [Au 25 (SCH 3 ) 18 ] -1 nanocluster to understand how independent electron and hole relaxations contribute to the overall relaxation dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Dilute Alloys Based on Au, Ag, or Cu for Efficient Catalysis: From Synthesis to Active Sites

The development of new catalyst materials for energy-efficient chemical synthesis is critical as over 80% of industrial processes rely on catalysts, with many of the most energy-intensive processes specifically using heterogeneous catalysis. Catalytic performance is a complex interplay of phenomena involving temperature, pressure, gas composition, surface composition and structure over multiple length and time scales. In response to this complexity, the integrated approach to heterogeneous dilute-alloy catalysis reviewed here brings together materials synthesis, mechanistic surface chemistry, reaction kinetics, in-situ and operando characterization, and theoretical calculations in a coordinated effort to develop design principles to predict and improve catalytic selectivity. Dilute alloy catalysts—in which isolated atoms or small ensembles of the minority metal on the host metal lead to enhanced reactivity while retaining selectivity—are particularly promising as selective catalysts. Several dilute alloy materials using Au, Ag and Cu as the majority host element, including more recently introduced support-free nanoporous metals and oxide-supported nanoparticle "raspberry colloid templated (RCT)" materials, are reviewed for selective oxidation and hydrogenation reactions. Progress in understanding how such dilute alloy catalysts can be used to enhance selectivity of key synthetic reactions is reviewed, including quantitative scaling from model studies to catalytic conditions. The dynamic evolution of catalyst structure and composition studied in surface science and catalytic conditions and their relationship to catalytic function are also discussed, followed by advanced characterization and theoretical modeling that have been developed to determine the distribution of minority metal atoms at or near the surface. Furthermore, the integrated approach demonstrates the success of bridging the divide between fundamental knowledge and design of catalytic processes in complex catalytic systems, which can accelerate the development of new and efficient catalytic processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Dual Protective Mechanism of AlPO 4 Coating on High-Nickel Cathode Material for High Energy Density and Long Cycle Life Lithium-Ion Batteries

Cathode material with high nickel content is a promising candidate for the future generation of Li-ion batteries (LIBs). However, severe structural degradation during cycling limits its practical use, especially for electric vehicles. Herein, AlPO 4 nanoparticles were synthesized and then coated onto the surface of a high-nickel layer-structured cathode via a dry coating method. The AlPO 4 nanoparticles coating significantly improved the cycling stability from 69.2% to over 80% capacity retention after 140 cycles. Furthermore, the structure and chemical composition of the AlPO 4 -coated cathode was investigated by XRD, SEM, XPS, and STEM. Compared with the non-coated cathode, we revealed a dual protective mechanism for enhanced cycling stability, where Al doping and Li 3 PO 4 coating play synergistic roles in protecting cathode material through long-term cycling. This work demonstrates a facile and environmentally friendly approach toward improving the performance of high-nickel LIB cathodes, which can be easily scaled up for industrial applications.

25 ENERGY STORAGE↗
DOE OSTI2020

Shape-Selective Mesoscale Nanoarchitectures: Preparation and Photocatalytic Performance

We create ordered arrays of shape-selective gold-titania composite nanomaterials at the mesoscale (100 µm to 5 mm) by a combination of both bottom-up and top-down approaches for exquisite control of the size, shape, and arrangement of nanomaterials. Lithographic techniques along with wet chemical synthetic methods were combined to create these composite nanomaterials. The photocatalytic activity of these TiO 2, TiO 2 -Au and SiO 2 -TiO 2 -Au nano-composite mesoscale materials was monitored by the photodegradation of a model analyte, methyl orange, under UV and visible (Vis) illumination. Bare TiO 2 - and SiO 2 -TiO 2 -coated pillar arrays showed significant activity toward methyl orange in UV light with degradation rates on the order of 10 −4 –10 −3 min −1 . The photocatalytic activity of these arrays was also found to depend on the nanoparticle shape, in which particles with more edges and corners were found to be more reactive than spherical particles (i.e., the photocatalytic activity decreased as follows: diamonds > squares > triangles > spheres). SiO 2 -TiO 2 -Au nano-composite pillar arrays were tested in both UV and Vis light and showed increased activity in Vis light but decreased activity in UV light as compared to the bare semiconductor arrays. Additionally, the Au nanorod-functionalized nanoarrays exhibit a strong shape-dependence in their photocatalytic activity toward methyl orange degradation in Vis light.

36 MATERIALS SCIENCE↗
DOE OSTI2021

AuPd Nanoicosahedra: Atomic-Level Surface Modulation for Optimization of Electrocatalytic and Photocatalytic Energy Conversion

Modulation of bimetallic nanocatalysts with atomic precision would allow for significant increases in catalyst activity through the optimization of heteroatomic interplay. In practice, this level of control over homogeneously turning the heteroatomic states in the surface regions of catalysts remains a great challenge for practical applications requiring mass production. In this work, a one-step aqueous strategy for preparation of AuPd nanoicosahedra core–shell structures has been developed. By turning the molar ratio of Au and Pd precursors, the nanoicosahedra could be made with uniform core composition (Pd ~20%) and largely flexible surface compositions (Pd: 20–70%). Under model reactions of electrochemical ethanol oxidation (EOR) and 4-nitrophenol (4-NP) reduction, the Au 55 Pd 45 surface displayed superior activities. Here, x-ray absorption spectroscopy revealed that AuPd nanoicosahedra with Pd-poor surfaces (Au 79 Pd 21 and Au 60 Pd 40 ) maintain Au-like electronic structures while those with Pd-rich surfaces are more Pd-like. The Au 55 Pd 45 surface struck a delicate balance between the two extremes, leading to the optimal Au–Pd interplay for catalytic performance. Overall, the development of a one-step aqueous strategy for atomic-level control over bimetallic nanoparticle surface states is an important milestone for future advances in catalysis. Our findings in atomic-scale catalyst design will bring deep insights into the fields of nanosynthesis and heterogeneous catalysis, which will be beneficial for further scientific breakthroughs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

An Overview of Nanomaterials for Environmental Remediation Applications

The environmental remediation capabilities of nanoparticles were reviewed and evaluated. Nanoparticles (NPs) have been used to remediate various forms of environmental contamination. Various materials, morphologies, and conditions are required to remediate different contaminants. Nanoparticles may have benefits and/or limitations compared with traditional remediation methods. New techniques are being applied to mitigate the limitations of NPs. Nanomaterials are a promising technology for the environmental remediation. NPs have been used for the remediation of aqueous and atmospheric contaminants. Nanoparticles have been used to sequester contaminants toxic to human and environmental health. Various materials, morphologies, and conditions are necessary for the remediation of different contaminants. The remediation of heavy metals is of significant concern. Contaminants may be remediated by means of sorption or reduction. The remediation capability of nanoparticles is promising due to their high surface area and reactivity. Reaction kinetics are, therefore, notably fast. These characteristics make NPs attractive for environmental remediation. Various NPs have been used as sequestering agents for environmental contaminants. NPs have been used to remediate heavy metals as well as organic contaminants. Technical Objectives: Assess viability of nanoparticles (NPs) for environmental remediation; Review benefits and limitations of NPs; Design future experiments to test remediation capabilities of NPs. Future Plans: Create NP filters for remediation - Grow Au NPs on Stainless Steel Wool: Stainless steel wool has many defects and crevices allowing the Au NPs to grow on the surface; Stainless steel wool will not react with the heavy metal contaminants tested; NPs are embedded, so they do not have to be removed from solution. Test sorption capabilities with heavy metal contaminants in aqueous solution. Benefits of Gold NPs: Corrosion/oxidation resistant; Exhibit visible/near IR plasmon resonance; Can be synthesized by solution chemistry: cost efficient and easily scalable. Surfactants: Used to lower surface energy and prevent aggregation; Sodium citrate: anionic surfactant (-); Cetyltrimethylammonium bromide (CTAB): cationic surfactant (+); Ionic surfactants create charged NPs; Charged NPs can be used to sequester ionic contaminants (eg. heavy metals)

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Adsorbate-induced adatom formation on Au-Cu bimetallic alloys and its possible consequences for CO 2 electroreduction

The adsorbate-induced formation of sub-nanometer clusters on transition-metal single crystals observed in previous high-pressure microscopic studies hinted at the in-situ formation of unique active sites even on large nanoparticle catalysts. We propose that the adatom formation energy can be used as an energetic descriptor for the initial step toward the adsorbate-induced metal-cluster formation process. This descriptor can be efficiently computed using density functional theory (DFT) calculations and applied for screening and identification of metal catalysts where this phenomenon may play an important role in generating active sites in-situ. As a proof of concept, here, we construct an adatom formation energy database for three Au x Cu y alloys (x:y = 3:1, 1:1, or 1:3) and eighteen adsorbates (H, C, N, O, F, S, Cl, Br, I, CH x , NH x (x = 1 – 3), CO, NO, and OH) commonly involved in catalytic reactions. The energetics of adatom formation were examined in all cases where the (111) terrace, (211) step-edge, and (874) kink were the sources of the adatom. We demonstrate that the presence of an adsorbate could alter not only the energetics for adatom formation but also the elemental nature of the preferred adatom being formed. Using our database, we identified promising systems which favor adsorbate-induced adatom formation under near-ambient conditions. Specifically, CO-induced adatom formation on all three Au-Cu alloy surfaces could occur under CO 2 electroreduction (CO 2 RR) conditions. This phenomenon offers a qualitative explanation for the experimentally observed CO 2 RR activity on Au-Cu alloy catalysts. As a result, our methodology offers an easily expandable and efficient approach for large-scale catalyst screening with regards to adatom/cluster formation under reaction conditions and provides insight into the possible nature of active sites on alloy catalysts from a novel perspective.

Active site↗
DOE OSTI2022

Impact of Surface Chemistry of Ultrasmall Superparamagnetic Iron Oxide Nanoparticles on Protein Corona Formation and Endothelial Cell Uptake, Toxicity, and Barrier Function

Ultrasmall superparamagnetic iron oxide nanoparticles (USPIONs) have been investigated for biomedical applications, including novel contrast agents, magnetic tracers for tumor imaging, targeted drug delivery vehicles, and magneto-mechanical actuators for hyperthermia and thrombolysis. Despite significant progress, recent clinical reports have raised concerns regarding USPION safety related to endothelial cell dysfunction; however, there is limited information on factors contributing to these clinical responses. The influence of USPION surface chemistry on nanoparticle interactions with proteins may impact endothelial cell function leading to adverse responses. Therefore, the goal of this study was to assess the effects of carboxyl-functionalized USPION (CU) or amine-functionalized USPION (AU) (approximately 30 nm diameter) on biological responses in human coronary artery endothelial cells. Increased protein adsorption was observed for AU compared with CU after exposure to serum proteins. Exposure to CU, but not AU, resulted in a concentration-dependent decrease in cell viability and perinuclear accumulation inside cytoplasmic vesicles. Internalization of CU was correlated with endothelial cell functional changes under non-cytotoxic conditions, as evidenced by a marked decreased expression of endothelial-specific adhesion proteins (eg, vascular endothelial-cadherin and platelet endothelial cell adhesion molecule-1) and increased endothelial permeability. Evaluation of downstream signaling indicated endothelial permeability is associated with actin cytoskeleton remodeling, possibly elicited by intracellular events involving reactive oxygen species, calcium ions, and the nanoparticle cellular uptake pathway. This study demonstrated that USPION surface chemistry significantly impacts protein adsorption and endothelial cell uptake, viability, and barrier function. This information will advance the current toxicological profile of USPION and improve development, safety assessment, and clinical outcomes of USPION-enabled medical products.

Toxicology↗